随着微电子技术的快速发展，电子元器件和集成电路的体积日益缩小与运行频率及功率密度的不断提升之间的矛盾导致单位面积的热流密度急剧飙升，温升造成的及时散热问题已成为制约电子器件发展及服役寿命的关键因素。为确保电子元器件的长期可靠稳定运行，开发综合性能优异的高导热绝缘复合材料至关重要。导热聚合物复合材料因具备良好的电绝缘和力学性能、稳定的化学性能、设计自由度大、易加工且成本低等优势，在微电子、电气绝缘、航空航天、太阳能等领域获得广泛应用。然而，当前导热聚合物复合材料面临着热导率(k)与介电强度(E_b)之间难以协同调控及同步提升的问题，严重限制了其在功率电子及高压电力绝缘设备等领域的应用。通过提高无序聚合物的分子链的结构有序性来实现本征导热性能的提升策略，不仅能同步提高k和E_b，还能保留其他优异性能，是解决当前导热聚合物复合材料面临难题的关键。

基于分子链间非共价作用及链取向调控聚合物链构象与空间排布的策略可构建多尺度有序结构，为声子传递提供高速通道，同步引入陷阱和抑制载流子迁移，实现解耦调控和同步提升k和E_b的目标。研究聚焦于三类链间作用力(金属-有机配位作用、π-π作用、偶极-偶极静电作用)与静电纺丝对聚合物结构及导热与绝缘强度的影响机制，实现对k和E_b性能的调控。研究内容包括：

(1) 以三价铬离子(Cr³⁺)、二价镉离子(Cd²⁺)和二价铜离子(Cu²⁺)为金属离子源调控聚乙烯醇(PVA)分子链结构的研究。结果发现，PVA的羟基与Cr³⁺、Cd²⁺、Cu²⁺的空轨道能够形成配位键，诱导分子链围绕金属离子做定向紧密排列，形成局部有序结构而促进声子传递。低离子含量下配位网络构建了连续的声子传输通道，过高含量则会引入界面缺陷与声子散射位点，导致热导率下降。当金属离子含量为1%时，k的排序为0.814 (Cr³⁺/PVA) > 0.685 (Cu²⁺/PVA) > 0.554 (Cd²⁺/PVA) >0.225 (PVA) W/(m·K)。离子调控的导热PVA依然保留了良好介电性能与高场击穿强度。

(2) 以含芳香环的聚醚酰亚胺(PEI)为对象，通过溶液流延法(SC-PEI)、静电纺丝高温压制(HP-PEI)工艺分别制备了PEI薄膜。研究发现，HP-PEI在150 °C能承受的最大E_b为400 MV/m，较SC-PEI的350 MV/m提升了14.3%，储能密度(U_e)达到2.71 J/cm³，相比SC-PEI (1.32 J/cm³)的提高了108%。HP-PEI的k值达0.68 W/(m·K)，相比SC-PEI (0.21 W/(m·K))提高了223.8%；红外热成像与COMSOL模拟进一步证实良好的散热性能。HP-PEI的k和E_b的同步提升源于纺丝诱导分子链取向与π-π堆叠作用协同构筑多尺度有序结构，声子传输路径得到优化。为了进一步提高k和E_b，在PEI中引入氮化硼纳米片(BNNS)后，1% BNNS/PEI的E_b和U_e分别达575 MV/m和4.76 J/cm³，k值高达0.77 W/(m·K)，归因于高导热绝缘BNNS片层有效阻挡载流子迁移，抑制电树枝的生长，BNNS协同PEI基体的有序结构进一步促进声子传递。

(3) 将PEI与聚酰亚胺(PI)共混，利用醚键(C-O-C)与酰亚胺基团(C=O、C-N-C)间的偶极-偶极作用诱导分子链紧密堆砌，通过静电纺丝-热压工艺制备PEI/PI共混膜。研究表明，4/6质量共混比下的PEI/PI薄膜在150 °C下的E_b达到625 MV/m，相比于纯PEI (400 MV/m)和纯PI (350 MV/m)得到显著提升，其U_e达到4.73 J/cm³，相比纯PEI (U_e=2.71 J/cm³)和纯PI (U_e=2.12 J/cm³)分别提高了73.3%和123.2%，且η保持在67%以上。PEI/PI膜的k值为0.86 W/(m·K)，相比同等条件制备的PEI (0.68 W/(m·K))的提高了26.8%。k和E_b协同提升归因于静电纺丝诱导链取向与偶极作用诱导的多尺度有序分子链结构同步促进声子传递及抑制载流子输运。引入1% BNNS-PEI/PI的E_b和U_e分别为825 MV/m和5.79 J/cm³，k值0.98 W/(m·K)，BNNS抑制漏导电流与电树枝化，减少声子散射，进一步提升了E_b和k。

该研究揭示了“链间非共价键与分子链取向对声子/载流子传输”的协同调控规律，为面向柔性电子、航空航天等极端环境的高性能导热材料的设计与制备提供了解决方案。

With the rapid advancement of microelectronics technology, the continuous miniaturization of electronic components and integrated circuits, coupled with increasing operating frequencies and power densities, has resulted in a dramatic rise in heat flux density per unit area. Thermal issues arising from localized temperature elevation have emerged as a critical bottleneck limiting both the development and operational lifespan of electronic devices. To ensure long-term reliability and stability of electronic components, the development of thermally conductive insulating composites with superior comprehensive performance is imperative. Owing to their exceptional electrical insulation, mechanical robustness, chemical stability, design versatility, processability, and cost-effectiveness, thermally conductive polymer composites have found extensive applications in microelectronics, electrical insulation systems, aerospace engineering, and solar energy technologies. However, existing composites face significant challenges in achieving concurrent enhancement and synergistic optimization of thermal conductivity (k) and dielectric breakdown strength (E_b), severely limiting their utility in high-power electronics and high-voltage insulation systems. A promising strategy involves enhancing the intrinsic thermal conductivity of amorphous polymers by improving the structural ordering of molecular chains. This approach not only enables simultaneous improvement of k and E_b but also retains other advantageous material properties, thereby offering a viable solution to the current limitations of thermally conductive polymer composites.

Strategies utilizing non-covalent intermolecular interactions and chain alignment can regulate polymer chain conformation and spatial arrangement, thereby constructing multiscale ordered structures that establish efficient phonon transport pathways. Concurrently, the introduction of charge traps and suppression of carrier migration enable decoupled control and simultaneous enhancement of k and E_b. This dissertation systematically investigates the mechanistic effects of three intermolecular interaction types (metal-organic coordination, π-π stacking, and dipole-dipole interactions), combined with electrospinning technology, on polymer structural evolution and its resultant thermal and dielectric properties, with the objective of achieving precise regulation of k and E_b. The main contents are as follows:

(1) Polyvinyl alcohol (PVA) was selected as a model polymer to investigate the regulation of its molecular chain structure using trivalent chromium (Cr³⁺), divalent cadmium (Cd²⁺), and divalent copper (Cu²⁺) ions as coordination centers. Results showed that the hydroxyl groups of PVA can form coordination bonds with the vacant orbitals of Cr³⁺, Cd²⁺, and Cu²⁺, inducing the directional and compact arrangement of molecular chains around the metal ions and forming locally ordered structures that facilitate phonon transport. At low ion concentrations, the coordination network establishes continuous phonon transport pathways, whereas excessive ion loading introduces interfacial defects and phonon scattering sites, leading to reduced thermal conductivity. At a 1% metal ion concentration, the k was ranked as follows: 0.814 (Cr³⁺/PVA) > 0.685 (Cu²⁺/PVA) > 0.554 (Cd²⁺/PVA) > 0.225 (PVA) W/(m·K). The ion-modified thermally conductive PVA also retained good dielectric performance and high dielectric breakdown strength.

(2) Polyetherimide (PEI), containing aromatic rings, was used to prepare films via solution casting (SC-PEI) and electrospinning followed by hot pressing (HP-PEI). The results showed that the breakdown strength of HP-PEI at 150 °C increased to 400 MV/m compared to 350 MV/m for SC-PEI, and its energy storage density (U_e) reached 2.71 J/cm³, representing a 108% improvement over SC-PEI (1.32 J/cm³). The k of HP-PEI reached 0.68 W/(m·K), a 223.8% increase over SC-PEI (0.21 W/(m·K)). Infrared thermography and COMSOL simulations further confirmed the excellent heat dissipation performance. The simultaneous enhancement in k and E_b is attributed to the multiscale ordered structures formed through the synergistic effect of chain orientation induced by electrospinning and π-π stacking between polymer chains. Furthermore, the incorporation of boron nitride nanosheets (BNNS) significantly enhanced properties. At 1 wt% BNNS loading, the PEI composite exhibited an E_b of 575 MV/m and U_e of 4.76 J/cm³, with k increasing to 0.77 W/(m·K), attributed to BNNS’s high thermal conductivity and insulating nature, which effectively blocks charge carrier migration, suppresses leakage current and electrical treeing, and promotes phonon transport in cooperation with the ordered polymer matrix.

(3) A PEI/polyimide (PI) blend was prepared using electrospinning-hot pressing, leveraging the dipole-dipole interactions between ether bonds (C-O-C) and imide groups (C=O, C-N-C) to induce compact molecular chain stacking. The PEI/PI film with a 4:6 blend ratio exhibited an E_b of 625 MV/m at 150 °C, significantly higher than pure PEI (400 MV/m) and pure PI (350 MV/m). The U_e reached 4.73 J/cm³, which represents improvements of 73.3% and 123.2% over pure PEI (2.71 J/cm³) and pure PI (2.12 J/cm³), respectively, with an efficiency (η) above 67%. The k of the PEI/PI film reached 0.86 W/(m·K), a 26.8% increase compared to HP-PEI under the same conditions (0.68 W/(m·K)). The synergistic enhancement of k and E_b is attributed to the electrospinning-induced chain orientation and dipole-dipole interactions forming multiscale ordered molecular structures that simultaneously promote phonon transport and suppress charge carrier movement. Incorporation of 1 wt% BNNS further elevated E_b and U_e to 825 MV/m and 5.79 J/cm³, respectively, with k reaching 0.98 W/(m·K), due to the BNNS’s ability to suppress leakage current and electrical treeing and reduce phonon scattering, thereby further enhancing both E_b and k.

This study elucidates the synergistic regulatory mechanism of non-covalent intermolecular interactions and polymer chain alignment in modulating phonon and charge carrier transport dynamics, offering critical insights for developing high-performance thermally conductive materials applicable to flexible electronics, aerospace systems, and other extreme-environment technologies.

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